Special Issue "Membranes for Lithium Batteries"

A special issue of Membranes (ISSN 2077-0375).

Deadline for manuscript submissions: closed (30 June 2018)

Special Issue Editor

Guest Editor
Dr. Giovanni Battista Appetecchi

ENEA (Italian National Agency for New Technologies, Energy and Sustainable Economic Development), Department for Sustainability (SSPT), Division for Sustainable Materials (PROMAS), Materials and Physicochemical Processes Laboratory (MATPRO), Casaccia Research Center, Via Anguillarese 301, 00123 Rome, Italy
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Interests: research and development of electrolyte/electrode materials/components for electrochemical energy storage systems; ionic liquids; polymer and gel electrolytes; lithium batteries

Special Issue Information

Dear Colleagues,

It is with great pleasure that we open a Special Issue on "Membranes for Lithium Batteries", fully focused on ionically conducting membranes as electrolytes for rechargeable lithium battery systems. The latter represents an excellent choice as next generation electrochemical storage devices due to their high energy density and cycling behavior. However, safety drawbacks mainly due to the electrolyte have prevented their development and commercialization, so far, in large-scale applications as automotive and storage from renewable power sources.

One of the most promising approaches to overcome these limitations is the adoption of Li+ ion conducting polymer membranes or polymer electrolytes (PEs), which represent a breakthrough for the realization of safer and high energy density electrochemical devices. Additionally, the development of PEs is undoubtedly appealing from the engineering point of views. They can be easily and cheaply manufactured into low thicknesses and shapes not allowed for supported liquid electrolytes, offering a new concept of all-solid-state, thin-layer, flexible (both mechanically and in design), robust, lithium polymer battery. In addition to their main role as the electrolytes, polymer electrolytes play a second role in composite electrode as binders and ionic conductors.

Understanding the formation and the transport properties of polymer electrolytes is not a simple matter, requiring strong interconnection between the polymer science and solid-state chemistry and traditionally concerned with inorganic compounds and crystal structures. Another key parameters are electrochemical stability and interfacial compatibility towards electrodes, which play starring roles in determining the battery performance.

The Special Issue, "Membranes for Lithium Batteries", is open to manuscripts focused on various issues (ion transport, thermal and electrochemical properties, compatibility towards electrodes, tests in battery) regarding ionically conducting polymer membranes to be tailored as electrolyte separators for solid-state lithium battery systems. Researchers and experts in these topics are warmly invited to submit their welcome articles.

Dr. Giovanni Battista Appetecchi
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All papers will be peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Membranes is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1000 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • polymer hosts
  • polymer electrolyte separators
  • gel electrolytes
  • lithium polymer batteries

Published Papers (6 papers)

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Research

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Open AccessArticle Gel Polymer Electrolytes Based on Silica-Added Poly(ethylene oxide) Electrospun Membranes for Lithium Batteries
Membranes 2018, 8(4), 126; https://doi.org/10.3390/membranes8040126
Received: 17 October 2018 / Revised: 27 November 2018 / Accepted: 30 November 2018 / Published: 5 December 2018
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Abstract
Solid polymer electrolytes, in the form of membranes, offering high chemical and mechanical stability, while maintaining good ionic conductivity, are envisaged as a possible solution to improve performances and safety in different lithium cell configurations. In this work, we designed and prepared systems [...] Read more.
Solid polymer electrolytes, in the form of membranes, offering high chemical and mechanical stability, while maintaining good ionic conductivity, are envisaged as a possible solution to improve performances and safety in different lithium cell configurations. In this work, we designed and prepared systems formed using innovative nanocomposite polymer membranes, based on high molecular weight poly(ethylene oxide) (PEO) and silica nanopowders, produced by the electrospinning technique. These membranes were subsequently gelled with solutions based on aprotic ionic liquid, carbonate solvents, and lithium salt. The addition of polysulfide species to the electrolyte solution was also considered, in view of potential applications in lithium-sulfur cells. The morphology of the electrospun pristine membranes was evaluated using scanning electron microscopy. Stability and thermal properties of pristine and gelled systems were investigated uisng differential scanning calorimetry and thermal gravimetric analysis. Electrochemical impedance spectroscopy was used to determine the conductivity of both swelling solutions and gelled membranes, allowing insight into the ion transport mechanism within the proposed composite electrolytes. Full article
(This article belongs to the Special Issue Membranes for Lithium Batteries)
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Open AccessArticle Composite Gel Polymer Electrolytes Based on Organo-Modified Nanoclays: Investigation on Lithium-Ion Transport and Mechanical Properties
Received: 26 July 2018 / Revised: 18 August 2018 / Accepted: 21 August 2018 / Published: 24 August 2018
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Abstract
Composite gel polymer electrolytes (GPEs) based on organo-modified montmorillonite clays have been prepared and investigated. The organo-clay was prepared by intercalation of CTAB molecules in the interlamellar space of sodium smectite clay (SWy) through a cation-exchange reaction. This was used as nanoadditive in [...] Read more.
Composite gel polymer electrolytes (GPEs) based on organo-modified montmorillonite clays have been prepared and investigated. The organo-clay was prepared by intercalation of CTAB molecules in the interlamellar space of sodium smectite clay (SWy) through a cation-exchange reaction. This was used as nanoadditive in polyacrylonitrile/polyethylene-oxide blend polymer, lithium trifluoromethanesulphonate (LiTr) as salt and a mixture of ethylene carbonate/propylene carbonate as plasticizer. GPEs were widely characterized by DSC, SEM, and DMA, while the ion transport properties were investigated by AC impedance spectroscopy and multinuclear NMR spectroscopy. In particular, 7Li and 19F self-diffusion coefficients were measured by the pulse field gradient (PFG) method, and the spin-lattice relaxation times (T1) by the inversion recovery sequence. A complete description of the ions dynamics in so complex systems was achieved, as well as the ion transport number and ionicity index were estimated, proving that the smectite clay surfaces are able to “solvatate” both lithium and triflate ions and to create a preferential pathway for ion conduction. Full article
(This article belongs to the Special Issue Membranes for Lithium Batteries)
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Open AccessArticle High Performance Polymer/Ionic Liquid Thermoplastic Solid Electrolyte Prepared by Solvent Free Processing for Solid State Lithium Metal Batteries
Received: 6 July 2018 / Revised: 25 July 2018 / Accepted: 26 July 2018 / Published: 2 August 2018
Cited by 3 | PDF Full-text (1771 KB) | HTML Full-text | XML Full-text
Abstract
A polymer/ionic liquid thermoplastic solid electrolyte based on poly(ethylene oxide) (PEO), modified sepiolite (TPGS-S), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and 1-Butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PYR14TFSI) ionic liquid is prepared using solvent free extrusion method. Its physical-chemical, electrical, and electrochemical properties are comprehensively studied. The investigated [...] Read more.
A polymer/ionic liquid thermoplastic solid electrolyte based on poly(ethylene oxide) (PEO), modified sepiolite (TPGS-S), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and 1-Butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PYR14TFSI) ionic liquid is prepared using solvent free extrusion method. Its physical-chemical, electrical, and electrochemical properties are comprehensively studied. The investigated solid electrolyte demonstrates high ionic conductivity together with excellent compatibility with lithium metal electrode. Finally, truly Li-LiFePO4 solid state coin cell with the developed thermoplastic solid electrolyte demonstrates promising electrochemical performance during cycling under 0.2 C/0.5 C protocol at 60 °C. Full article
(This article belongs to the Special Issue Membranes for Lithium Batteries)
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Open AccessArticle Ionic Liquid-Based Electrolyte Membranes for Medium-High Temperature Lithium Polymer Batteries
Received: 11 June 2018 / Revised: 4 July 2018 / Accepted: 9 July 2018 / Published: 10 July 2018
Cited by 2 | PDF Full-text (4109 KB) | HTML Full-text | XML Full-text
Abstract
Li+-conducting polyethylene oxide-based membranes incorporating N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide are used as electrolyte separators for all-solid-state lithium polymer batteries operating at medium-high temperatures. The incorporation of the ionic liquid remarkably improves the thermal, ion-transport and interfacial properties of the polymer [...] Read more.
Li+-conducting polyethylene oxide-based membranes incorporating N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide are used as electrolyte separators for all-solid-state lithium polymer batteries operating at medium-high temperatures. The incorporation of the ionic liquid remarkably improves the thermal, ion-transport and interfacial properties of the polymer electrolyte, which, in combination with the wide electrochemical stability even at medium-high temperatures, allows high current rates without any appreciable lithium anode degradation. Battery tests carried out at 80 °C have shown excellent cycling performance and capacity retention, even at high rates, which are never tackled by ionic liquid-free polymer electrolytes. No dendrite growth onto the lithium metal anode was observed. Full article
(This article belongs to the Special Issue Membranes for Lithium Batteries)
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Review

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Open AccessReview Review of Recent Nuclear Magnetic Resonance Studies of Ion Transport in Polymer Electrolytes
Membranes 2018, 8(4), 120; https://doi.org/10.3390/membranes8040120
Received: 18 September 2018 / Revised: 16 November 2018 / Accepted: 20 November 2018 / Published: 30 November 2018
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Abstract
Current and future demands for increasing the energy density of batteries without sacrificing safety has led to intensive worldwide research on all solid state Li-based batteries. Given the physical limitations on inorganic ceramic or glassy solid electrolytes, development of polymer electrolytes continues to [...] Read more.
Current and future demands for increasing the energy density of batteries without sacrificing safety has led to intensive worldwide research on all solid state Li-based batteries. Given the physical limitations on inorganic ceramic or glassy solid electrolytes, development of polymer electrolytes continues to be a high priority. This brief review covers several recent alternative approaches to polymer electrolytes based solely on poly(ethylene oxide) (PEO) and the use of nuclear magnetic resonance (NMR) to elucidate structure and ion transport properties in these materials. Full article
(This article belongs to the Special Issue Membranes for Lithium Batteries)
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Open AccessReview Recent Advances in Poly(vinylidene fluoride) and Its Copolymers for Lithium-Ion Battery Separators
Received: 29 June 2018 / Revised: 11 July 2018 / Accepted: 12 July 2018 / Published: 19 July 2018
Cited by 8 | PDF Full-text (8385 KB) | HTML Full-text | XML Full-text
Abstract
The separator membrane is an essential component of lithium-ion batteries, separating the anode and cathode, and controlling the number and mobility of the lithium ions. Among the polymer matrices most commonly investigated for battery separators are poly(vinylidene fluoride) (PVDF) and its copolymers poly(vinylidene [...] Read more.
The separator membrane is an essential component of lithium-ion batteries, separating the anode and cathode, and controlling the number and mobility of the lithium ions. Among the polymer matrices most commonly investigated for battery separators are poly(vinylidene fluoride) (PVDF) and its copolymers poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE), poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and poly(vinylidene fluoride-cochlorotrifluoroethylene) (PVDF-CTFE), due to their excellent properties such as high polarity and the possibility of controlling the porosity of the materials through binary and ternary polymer/solvent systems, among others. This review presents the recent advances on battery separators based on PVDF and its copolymers for lithium-ion batteries. It is divided into the following sections: single polymer and co-polymers, surface modification, composites, and polymer blends. Further, a critical comparison between those membranes and other separator membranes is presented, as well as the future trends on this area. Full article
(This article belongs to the Special Issue Membranes for Lithium Batteries)
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